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This thesis focuses on understanding the chemistry involved in a variety of surface modification reactions, both on metal oxides and graphene. In this work, the rates of chemisorption of a prototypical phosphonic acid on ITO under several processing protocols are measured using XPS to determine the optimal procedure. UPS is used to track the dependence of the electronic structure of the system, specifically of the work function and position of the valence band maximum on coverage. Phosphonic acid monolayers with appropriate tail groups can also be used to initiate chemistry from surfaces, which has potential for building layers of organic-electronic devices, including organic solar cells and capacitors. The growth of non-conjugated polymers from BaTiO₃ nanoparticles using a facile ATRP technique is studied via solution-phase and solid-state techniques to determine its applicability to make matrix-free composites for hybrid dielectrics. In addition, the surface chemistry involved in Kumada Catalyst-Transfer to grow polythiophene derivatives from ITO is examined via XPS. Finally, the newly emerged alternative for replacement of ITO as transparent electrode, graphene, is n- and p-doped using redox-active, solution-processable metal-organics, which increased its conductivity and allowed the work function to be tuned over a range of 1.8 eV. The systems are characterized in a systematic study, and the results are promising for future applications of graphene.